Hydrazine‐Assisted Acidic Water Splitting Driven by Iridium Single Atoms

Abstract Water splitting, an efficient technology to produce purified hydrogen, normally requires high cell voltage (>1.5 V), which restricts the application of single atoms electrocatalyst in water oxidation due to the inferior stability, especially in acidic environment. Substitution of anodic oxygen evolution reaction (OER) with hydrazine oxidation reaction (HzOR) effectually reduces the overall voltage. In this work, the utilization of iridium single atom (Ir‐SA/NC) as robust hydrogen evolution reaction (HER) and HzOR electrocatalyst in 0.5 m H 2 SO 4 electrolyte is reported. Mass activity of Ir‐SA/NC is as high as 37.02 A mg Ir −1 at overpotential of 50 mV in HER catalysis, boosted by 127‐time than Pt/C. Besides, Ir‐SA/NC requires only 0.39 V versus RHE to attain 10 mA cm −2 in HzOR catalysis, dramatically lower than OER (1.5 V versus RHE); importantly, a superior stability is achieved in HzOR. Moreover, the mass activity at 0.5 V versus RHE is enhanced by 83‐fold than Pt/C. The in situ Raman spectroscopy investigation suggests the HzOR pathway follows *N 2 H 4 →*2NH 2 →*2NH→2N→*N 2 →N 2 for Ir‐SA/NC. The hydrazine assisted water splitting demands only 0.39 V to drive, 1.25 V lower than acidic water splitting.